US4780796A - Solid electrolytic capacitor - Google Patents
Solid electrolytic capacitor Download PDFInfo
- Publication number
- US4780796A US4780796A US07/138,591 US13859187A US4780796A US 4780796 A US4780796 A US 4780796A US 13859187 A US13859187 A US 13859187A US 4780796 A US4780796 A US 4780796A
- Authority
- US
- United States
- Prior art keywords
- electrically conductive
- electrolytic capacitor
- conductive polymer
- polymer layer
- polypyrrole
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Expired - Lifetime
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Classifications
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G4/00—Fixed capacitors; Processes of their manufacture
- H01G4/002—Details
- H01G4/018—Dielectrics
- H01G4/06—Solid dielectrics
- H01G4/08—Inorganic dielectrics
- H01G4/12—Ceramic dielectrics
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
- H01G9/004—Details
- H01G9/022—Electrolytes; Absorbents
- H01G9/025—Solid electrolytes
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/22—Electrodes
- H01G11/30—Electrodes characterised by their material
- H01G11/48—Conductive polymers
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/54—Electrolytes
- H01G11/56—Solid electrolytes, e.g. gels; Additives therein
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
- H01G9/004—Details
- H01G9/02—Diaphragms; Separators
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
- H01G9/004—Details
- H01G9/022—Electrolytes; Absorbents
- H01G9/025—Solid electrolytes
- H01G9/028—Organic semiconducting electrolytes, e.g. TCNQ
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/13—Energy storage using capacitors
Definitions
- the present invention relates to a solid electrolytic capacitor that utilizes an electrically conductive polymer as a solid electrolyte.
- capacitors which have excellent high-frequency characteristics include thin-film, mica and ceramic capacitors. These conventional capacitors, however, involve the problem that, when they are designed to obtain an electrostatic capacity of 1 ⁇ F or more, their size is increased, and the production cost is also raised considerably.
- Electrolytic capacitors which are known to be large-capacity capacitors include two types, that is, the liquid electrolyte type in which a liquid electrolyte is impregnated, and the solid electrolyte type in which manganese dioxide is employed as a solid electrolyte.
- the former type of electrolytic capacitor which employs an electrolyte in a liquid state utilizes ion conduction, and there is therefore a remarkably increased resistance in the high-frequency region, whereby the impedance of the capacitor increases disadvantageously.
- the latter type of electrolytic capacitor employs as a solid electrolyte manganese dioxide and a charge transfer complex consisting of a combination of 7,7,8,8-tetracyanoquinodimethane (hereinafter referred to as TCNQ) and an electron donor.
- TCNQ 7,7,8,8-tetracyanoquinodimethane
- the type of electrolytic capacitor which employs manganese dioxide as a solid electrolyte is obtained by thermally decomposing manganese nitrate since manganese dioxide is an insoluble solid substance.
- This type of electrolytic capacitor also has relatively high impedance in the high-frequency region, partly because manganese dioxide has a relatively high specific resistance, and partly because it is subjected to thermal decomposition several times to obtain manganese dioxide. Also a dielectric oxide coating provided on this type of electrolytic capacitor may be readily damaged, and the loss current of the capacitor thus increases to a remarkable extent.
- a type of electrolytic capacitor which employs as a solid electrolyte a hetrocyclic polymer obtained by a electrochemical polymerization method has been proposed in recent years (see Japanese patent public disclosure No. 244017/1985, No. 2315/1986).
- the electrolytic capacitor described above comprises an electrode having a dielectric oxide coating thereon and a solid electrolyte consisting of an electrically conductive hetrocyclic polymer which is formed by an electrochemical oxidation method.
- a solid electrolyte consisting of an electrically conductive hetrocyclic polymer which is formed by an electrochemical oxidation method.
- forming the electrically conductive hetrocyclic polymer on the dielectric oxide coating is impossible or, at least, difficult because the dielectric oxide coating is an insulator.
- an electrically conductive polymer is formed by a chemical oxidation method or an electrochemical oxidation method.
- the polymer which is obtained by the former method has poor mechanical strength.
- No polymer is formed on the dielectric oxide coating using the latter method because the dielectric oxide coating is an insulator.
- FIG. 1 is a schematic, partial, sectional view illustrating the construction of a solid electrolytic capacitor according to one embodiment of the present invention.
- a solid electrolytic capacitor comprising, in combination, an electrode having an adherent dielectric oxide coating thereon and a solid electrolyte comprising both an electrically conductive polymer layer (I) which is formed by a chemical oxidation method, contacting a monomer with an oxidizing agent, and an electrically conductive polymer layer (II) which is formed by electrochemical oxidation method.
- FIG. 1 partially shows the construction of an electrical capacitor which embodies the present invention.
- the surface of an electrode 1 which is roughened by an electrochemical treatment is oxidized by an electrochemical oxidation treatment or an air oxidation treatment whereby a dielectric oxide coating 2 is formed on the electrode.
- a solution containing an oxidizing agent in a concentration of 0.001 mol/l to 2 mol/l is dispersed uniformly on the dielectric oxide coating by dipping, coating or spraying and the oxidizing agent is then brought into contact with a monomer of an electrically conductive polymer (I) or a solution of the monomer in a concentration of more than 0.01 mol/l. Consequently, an electrically conductive polymer layer 3 which is obtained by a chemical oxidation method is formed on the dielectric oxide coating 2.
- the electrically conductive polymer layer 3 is able to be formed by an inverse procedure in which the monomer is brought into contact with the oxidizing agent.
- the electrically conductive polymer layer 3 is used as an anode for electro polymerization.
- An electrically conductive polymer layer 4 which is obtained by an electrochemical oxidation method is formed in a cell containing a solution of a monomer of an electrically conductive polymer (II) in a concentration of 0.01 mol/l to 5 mol/l and an electrolyte salt in a concentration of 0.01 mol/l to 2 mol/l. Consequently, the electrically conductive polymer layer 4 is formed on the electrically conductive polymer layer 3.
- a counter electrode is brought into contact with the electrically conductive polymer layer 4 using an electrically conductive adhesive (silver paste etc.)
- the capacitor of the present invention is completed by the procedure described above and is then molded with epoxy resin.
- the electrode used in the capacitor of this invention is generally selected from either aluminum or tantalum.
- oxidizing agents include a halogen such as iodine, bromine and bromine iodide; a halide such as antimony pentafluoride, arsenic pentafluoride, silicon tetrafluoride, phosphorus pentachloride, phosphorus pentafluoride, feric-chloride, aluminum chloride and molybdenum chloride; a protonic acid such as sulfuric acid, nitric acid, fluorosulfuric acid, trifluoromethane sulfuric acid and chlorosulfuric acid; a compound containing oxygen such as sulfur trioxide, nitrogen dioxide and chlorine dioxide; a persulfate such as sodium persulfate, potassium persulfate and ammonium persulfate; and a peroxide such as hydrogen peroxide, peracetic acid and difluorosulfunil peroxide.
- a halogen such as iodine, bromine and bromine iodide
- the preferred compounds of said oxidizing agent are chlorine dioxide and ammonium persulfate.
- Said electrically conductive polymer layer (I) which is formed by a chemical oxidation method is generally selected from the group consisting of polypyrrole, polythiophene, polyaniline and polyfuran.
- the preferred polymer of said electrically conductive polymer layer (I) is polypyrrole or polyaniline.
- Said electrolyte salt consists of an anion and a cation.
- Commonly used anions include an halogenated anion such as hexafluorophosphate, hexafluoroarsenate, tetrafluoroborate and perchlorate; a halide such as chloride, bromide and iodide; and a sulfonate such as alkylbenzenesulfonate, aminobenzenesulfonate, benzenesulfonate and ⁇ -naphthalenesulfonate.
- the most preferred anion is sulfonate.
- Commonly used cations include an alkali metal cation such as lithium, sodium and potassium; and an ammonium cation such as ammonium and tetraalkilammonium.
- Suitable electrolyte salts include lithium hexafluorophosphate, lithium hexafluoroarsenate, lithium perchlorate, sodium iodide, sodium hexafluorophosphate, sodium perchlorate, potassium iodide, potassium hexafluorophosphate, potassium hexafluoroarsenate, potassium perchlorate, lithium tetrafluoroborate and tetrabutylammonium toluenesulfonate.
- Said electrically conductive polymer layer (II) which is formed by an electrochemical oxidation method is generally selected from the group consisting of polypyrrole, polythiophene, polyaniline and polyfuran.
- the most preferred electrically conductive polymer layer (II) is polypyrrole or polyaniline.
- an electric capacitor having a TCNQ charge transfer complex as an electrolyte has excellent high-frequency characteristics.
- the TCNQ charge transfer complex suffers from thermal stability and therefore involves a risk of the complex being decomposed during the capacitor manufacturing process to become an insulator.
- forming an electrically conductive hetrocyclic polymer having excellent mechanical strength by an electrochemical oxidation method on an electrode having a dielectric oxide coating is impossible, because the dielectric oxide coating is an insulator.
- This solid electrolytic capacitor having an organic semiconductor as a solid electrolyte is excellent in both electrical characteristics and thermal stability.
- An aluminium anode foil (thickness: 60 ⁇ m) having a dielectric aluminium oxide coating formed thereon by an electrochemical oxidation treatment was dipped in an aqueous solution containing 0.04 mol/l ammonium persulfate under reduced pressure conditions for 10 minutes and then dried.
- the anode foil was dipped in acetonitrile containing 2.0 mol/l pyrrole monomer under reduced pressure conditions for 10 minutes.
- a thin layer of polypyrrole was formed on the dielectric aluminium oxide coating by a chemical oxidation method.
- the anode foil was dipped in an aqueous solution containing 0.2 mol/l pyrrole monomer, 0.02 mol/l oxalic acid and 0.05 mol/l tetrabutylammonium toluene-sulfonate as an electrolyte.
- the anode foil was used as an anode and a stainless steel plate was used as a cathode.
- a uniform black layer of polypyrrole was formed galvanostatically on the anode foil under a current density of 0.5 mA/cm 2 applied for 150 minutes. After a counter electrode had been brought into contact with the black layer of polypyrrole using a silver paste, a capacitor was obtained and then molded with epoxy resin.
- Ethyl ether containing 0.1 mol/l iodine was sprayed on an aluminium anode foil (thickness: 60 ⁇ m) having a dielectric aluminium oxide coating formed thereon by an electrochemical oxidation treatment and the anode foil was then dried.
- Example 1 After dipping the anode foil in pyrrole monomer for 30 minutes under reduced pressure conditions, a black layer of polypyrrole was formed on the dielectric aluminium oxide coating by a chemical oxidation method. The following procedures were carried out in a similar manner to Example 1.
- An aluminium anode foil (thickness: 60 ⁇ m) having a dielectric aluminium oxide coating thereon was dipped in an aqueous solution containing 0.02 mol/l feric chloride for 2 minutes under reduced pressure conditions and then dried.
- An aluminium anode foil (thickness: 60 ⁇ m) having a dielectric aluminium oxide coating formed thereon by an electrochemical oxidation method was dipped in pyrrole monomer.
- a gaseous mixture containing 5 vol% chlorine dioxide was brought into contact with the anode foil for 5 minutes, a black layer of polypyrrole was formed on the dielectric aluminium oxide coating by a chemical oxidation method.
- the following procedures were carried out in a similar manner to Example 1.
- An electrochemical oxidation treatment was carried out similar to Example 1 except that a layer of polypyrrole was formed on a dielectric aluminium oxide coating by a chemical oxidation method. Polypyrrole was formed on only a part of the dielectric aluminium oxide coatingl and no uniform layer of polypyrrole was formed.
- An aluminium anode foil (thickness: 60 ⁇ m) having a dielectric aluminium oxide coating formed thereon by an electrochemical oxidation treatment was dipped in aniline monomer.
- the anode foil was dipped in an aqueous solution containing 1.0 mol/l aniline monomer and 1.0 mol/l sulfuric acid as an electrolyte.
- the anode foil was used as an anode and a platinum plate as a cathode.
- a uniform dark green layer of polyaniline was formed on the anode foil galvanostatically under a current density of 0.5 mA/cm 2 applied for 150 minutes.
- a counter electrode was brought into contact with the dark green layer of polyaniline using a silver paste, a capacitor was obtained and then molded with epoxy resin.
- a sintered tantalum anode pellet having a dielectric tantalum oxide coating formed thereon by an electrochemical oxidation treatment was dipped in an aqueous solution containing 0.04 mol/l ammonium persulfate under reduced pressure conditions for 5 minutes and then dried.
- the anode pellet was dipped in an aqueous solution containing 2.0 mol/l pyrrole monomer and 0.02 mol/l adipic acid under reduced pressure conditions for 10 minutes.
- a thin layer of polypyrrole was formed on the dielectric tantalum oxide by a chemical oxidationl method.
- the anode pellet was dipped in an aqueous solution containing 0.2 mol/l pyrrole monomer, 0.02 mol/l oxalic acid and 0.05 mol/l lithium perchlorate as an electrolyte.
- the anode pellet was used as an anode and a stainless steel plate as a cathode.
- a uniform black layer of polypyrrole was formed galvanostatically on the anode pellet under a current density of 0.5 mA/cm 2 applied for 150 minutes. After a counter electrode had been brought into contact with the black layer of polypyrrole using silver paste, a capacitor was obtained and then molded with epoxy resin.
- a sintered tantalum anode pellet having a dielectric tantalum oxide coating formed thereon by an electrochemical oxidation treatment was dipped in pyrrole monomer.
- Cap means electrostatic capacity at 120 Hz
- tan ⁇ means dielectric loss tangent at 120 Hz.
- Electrostatic capacity of the aluminium anode foil and the tantalum pellet used in Example show 2.0 ⁇ F/cm 2 and 1.0 ⁇ F, respectively, when an aqueous solution containing 50 g/l boric acid, 50 g/l citric acid and 50 ml/l ammonia water (28 wt%) is employed as liquid electrolyte.
Abstract
Description
TABLE 1 ______________________________________ Solid Electrical Characteristics Ex. Anode Electrolyte Cap (μF/cm.sup.2) tan δ (%) ______________________________________ 1 aluminium polypyrrole 2.2 1.5 2 aluminium polypyrrole 2.0 1.3 3 aluminium polypyrrole 2.1 1.8 4 aluminium polypyrrole 2.2 1.3 5 aluminium polyaniline 2.0 1.2 6 tantalum polypyrrole 1.2 1.0 7 tantalum polypyrrole 1.2 0.9 ______________________________________
Claims (5)
Applications Claiming Priority (4)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
JP61-4053 | 1987-01-13 | ||
JP62004053A JPS63173313A (en) | 1987-01-13 | 1987-01-13 | Solid electrolytic capacitor |
JP61-28197 | 1987-02-12 | ||
JP62028197A JPS63197319A (en) | 1987-02-12 | 1987-02-12 | Solid electrolytic capacitor |
Publications (1)
Publication Number | Publication Date |
---|---|
US4780796A true US4780796A (en) | 1988-10-25 |
Family
ID=26337759
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
US07/138,591 Expired - Lifetime US4780796A (en) | 1987-01-13 | 1987-12-28 | Solid electrolytic capacitor |
Country Status (4)
Country | Link |
---|---|
US (1) | US4780796A (en) |
EP (1) | EP0274755B1 (en) |
KR (1) | KR910009477B1 (en) |
DE (1) | DE3773166D1 (en) |
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Also Published As
Publication number | Publication date |
---|---|
DE3773166D1 (en) | 1991-10-24 |
EP0274755B1 (en) | 1991-09-18 |
EP0274755A2 (en) | 1988-07-20 |
KR880009402A (en) | 1988-09-15 |
EP0274755A3 (en) | 1988-10-05 |
KR910009477B1 (en) | 1991-11-16 |
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